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Here, we demonstrate the extension of two key components of high-harmonic spectroscopy, i.e., impulsive alignment and measurements with multiple driving wavelengths to 1,3-cyclohexadiene and benzene. In the case of 1,3-cyclohexadiene, we find that the temporal sequence of maximal and minimal emitted high-harmonic intensities as a function of the delay between the alignment and probe pulses inverts between 25 and 30\u2009eV and again between 35 and 40\u2009eV when an 800-nm driver is used, but no inversions are observed with a 1420-nm driver. This observation is explained by the wavelength-dependent interference of emission from multiple molecular orbitals (HOMO to HOMO-3), as demonstrated by calculations based on the weak-field asymptotic theory and accurate photorecombination matrix elements. These results indicate that attosecond charge migration takes place in the 1,3-cyclohexadiene cation and can potentially be reconstructed with the help of additional measurements. Our experiments also demonstrate a pathway toward studying photochemical reactions in the molecular frame of 1,3-cyclohexadiene.<\/jats:p>","DOI":"10.1063\/4.0000227","type":"journal-article","created":{"date-parts":[[2024,2,29]],"date-time":"2024-02-29T16:26:41Z","timestamp":1709224001000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":5,"title":["High-harmonic spectroscopy of impulsively aligned 1,3-cyclohexadiene: Signatures of attosecond charge migration"],"prefix":"10.1063","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-6502-197X","authenticated-orcid":false,"given":"Andres","family":"Tehlar","sequence":"first","affiliation":[{"name":"Laboratory of Physical Chemistry, ETH Z\u00fcrich 1 , 8093 Z\u00fcrich, Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0632-4981","authenticated-orcid":false,"given":"Jakob T.","family":"Casanova","sequence":"additional","affiliation":[{"name":"Laboratory of Physical Chemistry, ETH Z\u00fcrich 1 , 8093 Z\u00fcrich, Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9381-2133","authenticated-orcid":false,"given":"Andrey","family":"Dnestryan","sequence":"additional","affiliation":[{"name":"Moscow Institute of Physics and Technology 2 , Dolgoprudny 141700, Russia"},{"name":"National Research University Higher School of Economics 3 , Moscow 101000, Russia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4576-5838","authenticated-orcid":false,"given":"Frank","family":"Jensen","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Aarhus University 4 , 8000 Aarhus C, Denmark"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7403-2070","authenticated-orcid":false,"given":"Lars Bojer","family":"Madsen","sequence":"additional","affiliation":[{"name":"Department of Physics and Astronomy, Aarhus University 5 , 8000 Aarhus C, Denmark"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7603-2322","authenticated-orcid":false,"given":"Oleg I.","family":"Tolstikhin","sequence":"additional","affiliation":[{"name":"Moscow Institute of Physics and Technology 2 , Dolgoprudny 141700, Russia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8877-0872","authenticated-orcid":false,"given":"Hans Jakob","family":"W\u00f6rner","sequence":"additional","affiliation":[{"name":"Laboratory of Physical Chemistry, ETH Z\u00fcrich 1 , 8093 Z\u00fcrich, Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2024,2,29]]},"reference":[{"key":"2024022916263383200_c1","doi-asserted-by":"publisher","first-page":"867","DOI":"10.1038\/nature03183","volume":"432","year":"2004","journal-title":"Nature"},{"key":"2024022916263383200_c2","doi-asserted-by":"publisher","first-page":"103901","DOI":"10.1103\/PhysRevLett.102.103901","volume":"102","year":"2009","journal-title":"Phys. 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